Modulation of Charge Redistribution in Heterogeneous CoSe-Ni0.95Se Coupling with Ti3C2Tx MXene for Hydrazine-Assisted Water Splitting,Small

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Modulation of Charge Redistribution in Heterogeneous CoSe-Ni0.95Se Coupling with Ti3C2Tx MXene for Hydrazine-Assisted Water Splitting
Small ( IF 13.0 ) Pub Date : 2024-06-22 , DOI: 10.1002/smll.202403270
Zhongbao Feng _{1,

2,

3} , Haoyu Meng ₃ , Yumo Fu ₃ , Lili Ren ₄ , Bo Gao ₃ , Wentao Liu ₃

Affiliation

Integrating abundant dual sites of hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER) into one catalyst is extremely urgent toward energy-saving H₂ production. Herein, CoSe-Ni_0.95Se heterostructure coupling with Ti₃C₂T_x MXene (CoSe-Ni_0.95Se/MXene) is fabricated on nickel foam (NF) to enhance the catalytic performance. The heterogeneous CoSe-Ni_0.95Se and MXene coupling effect can change the coordination of Ni and Co, resulting in adjusted interfacial electronic field and enhanced electron transfer from Ni_0.95Se to CoSe especially near MXene surface. Also, the appearance of MXene can anchor more active sites, thereby abundant nucleophilic CoSe and electrophilic Ni_0.95Se are formed induced by the charge redistribution, which can tailor d-band center, moderate ^*H adsorption free energy (∆G_H^*) and facilitate adsorption/desorption for hydrazine intermediates, contributing to much enhanced HER and HzOR performance. For example, the low potentials of −160.8 and 116.1 mV at 400 mA cm⁻² are seen for HER and HzOR with long-term stability of 7 days. When assembled as overall hydrazine splitting (OHzS), a small cell voltage of 0.35 V to drive 100 mA cm⁻² is obtained. Such concept of integrating abundant nucleophilic and electrophilic dual sites and regulating their d-band centers can offer in-depth understandings to design efficient bifunctional HER and HzOR electrocatalysts.

中文翻译：

异质 CoSe-Ni0.95Se 与 Ti3C2Tx MXene 耦合中电荷再分布的调制用于肼辅助分解水

将丰富的肼氧化反应（HzOR）和析氢反应（HER）双位点整合到一个催化剂中，对于节能 H₂ 生产来说极为紧迫。在此，在泡沫镍（NF）上制备了 CoSe-Ni_0.95Se 异质结构与 Ti₃C₂T_x MXene （CoSe-Ni_0.95Se/MXene）的偶联，以增强催化性能。异质 CoSe-Ni_0.95Se 和 MXene 耦合效应可以改变 Ni 和 Co 的配位，从而调整界面电子场并增强从 Ni_0.95Se 到 CoSe 的电子转移，尤其是在 MXene 表面附近。此外，MXene 的出现可以锚定更多的活性位点，从而在电荷重新分布的诱导下形成丰富的亲核 CoSe 和亲电 Ni_0.95Se，这可以定制 d 带中心、适度的 ^*H 吸附自由能（∆G_H^*）并促进肼中间体的吸附/解吸，有助于大大提高 HER 和 HzOR 性能。例如，HER 和 HzOR 在 400 mA ^cm-2 时观察到 -160.8 和 116.1 mV 的低电位，长期稳定性为 7 天。当组装为整体肼分裂（OHzS）时，可获得 0.35 V 的小电池电压以驱动 100 mA cm⁻²。这种整合丰富的亲核和亲电双位点并调节它们的 d 带中心的概念可以为设计高效的双功能 HER 和 HzOR 电催化剂提供深入的理解。

更新日期：2024-06-22

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